CN104557368A - System for preparing ethylene, ethylene and arene from kinds of raw materials by coupling and transformation and method for system - Google Patents
System for preparing ethylene, ethylene and arene from kinds of raw materials by coupling and transformation and method for system Download PDFInfo
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Abstract
The invention relates to a system for preparing ethylene, ethylene and arene from kinds of raw materials by coupling and transformation and a method for the system, and mainly aims at solving the problems in the prior art that the raw material is single, the arene yield is low, and the product structure cannot be flexibly modulated according to the market requirements. The system comprises an aromatization reactor (1), a quench tower (2), a knockout tower (3) and a steam cracking unit (4); a product generated by the aromatization reactor (1) sequentially enters the quench tower (2) and the knockout tower (3); a gaseous product obtained by the knockout tower (3) enters a separation system of the steam cracking unit (4) through a compressor (5); and partial ethane (20), propane (21), C4 raffinate (27) and C5 and C6 non-arene (11), which are obtained by the knockout tower (3) and the separation system of the steam cracking unit (4) are returned to the aromatization reactor (1) as circulating materials. The problems are relatively well solved; and the system and the method can be applied to industrial production of ethylene, ethylene and arene.
Description
Technical field
The present invention relates to a kind of material coupled system and the method thereof transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type.
Background technology
Ethene, propylene and aromatic hydrocarbons (especially triphen, benzene Benzene, toluene Toluene, dimethylbenzene Xylene, i.e. BTX) are important basic organic synthesis raw materials.By the driving of downstream derivative thing demand, the market requirement sustainable growth of ethene, propylene and aromatic hydrocarbons.
The steam cracking process being raw material with liquid hydrocarbon (as petroleum naphtha, diesel oil, secondary processing oil) is the main production of ethene, propylene and aromatic hydrocarbons.This technique belongs to petroleum path production technology, and in recent years, the supply limited due to petroleum resources and higher price, raw materials cost constantly increases.The factor be subject to, alternative materials is prepared ethene, propylene and aromatic hydrocarbons technology and is caused and pay close attention to more and more widely.Wherein, for coal-based methanol, dme raw material, due to rich coal resources in China, become a kind of important Chemical Manufacture raw material just gradually, become the important supplement of petroleum.Therefore, consider in the production of ethene, propylene and aromatic hydrocarbons, introduce methyl alcohol, dme raw material, thus reduce raw materials cost, improve the market competitiveness and the ability to ward off risks.
In various existing methyl alcohol, dimethyl ether catalysis transformation technology, in the product of methanol/dimethyl ether aromatic hydrocarbons, comprise ethene, propylene and aromatic hydrocarbons simultaneously.This technology sees the people (Journal of Catalysis, 1977,47,249) such as the Chang of Mobil company in 1977 at first and reports on ZSM-5 molecular sieve catalyzer methyl alcohol and oxygenatedchemicals transforms the method preparing the hydrocarbon polymers such as aromatic hydrocarbons.1985, Mobil company is in its US Patent No. 1590321 of applying for, disclose the result of study of methyl alcohol, dimethyl ether conversion aromatic hydrocarbons first, this research adopt phosphorous be 2.7 % by weight ZSM-5 molecular sieve be catalyzer, temperature of reaction is 400 ~ 450 DEG C, methyl alcohol, dme air speed 1.3 (Grams Per Hour)/gram catalyzer.
Patent in methanol conversion for preparing arene catalyzer is more, as Chinese patent CN102372535, CN102371176, CN102371177, CN102372550, CN102372536, CN102371178, CN102416342, CN101550051, US Patent No. 4615995, US2002/0099249A1 etc.These patents are mainly around metal-modified ZSM-5 molecular sieve catalyzer, and modified metal comprises Zn, Ga, Ag, Cu, Mn etc.
US Patent No. 4686312, Chinese patent ZL101244969, ZL1880288, CN101602646, CN101823929, CN101671226, CN102199069, CN102199446, CN1880288 etc. disclose the operational path of multiple Methanol aromatic hydrocarbons.These patents product for the purpose of aromatic hydrocarbons, patent CN102775261, CN102146010, CN102531821, CN102190546, CN102372537 be other products such as co-producing light olefins, gasoline while Methanol aromatic hydrocarbons.
Wherein, disclosed in patent CN102775261, Multi-function methanol working method and device utilize preparing low carbon olefin hydrocarbon with methanol, gasoline, aromatic hydrocarbons.The method adopts two-step approach production technique, the first step methanol feedstock produces low-carbon alkene under special-purpose catalyst 1 acts on, reaction gas containing low-carbon alkene after heat exchange, chilling, carrying out washing treatment, is synthesized aromatic hydrocarbons and or gasoline by second step under the effect of special-purpose catalyst 2.The reactor of two reaction process can be fixed bed or fluidized-bed.The method adopts two-step approach, and technical process is complicated.
Take methyl alcohol as the technique of raw material production low-carbon alkene and arene parallel cogeneration gasoline disclosed in patent CN102146010.Be raw material with methyl alcohol and adopt molecular sieve catalyst to produce low-carbon alkene and arene parallel cogeneration gasoline through methyl alcohol alkylation reaction and aromatization.The reactor of methyl alcohol alkylation reaction and aromatization is various types of fixed-bed reactor, pressure 0.01 ~ 0.5 MPa, temperature 180 ~ 600 DEG C.Total liquid yield is greater than 70 % by weight, and triphen yield is greater than 90 % by weight.The method also adopts two reactors, and technical process is complicated.
Be the method for the co-fed production low-carbon alkene of methyl alcohol and petroleum naphtha and/or aromatic hydrocarbons disclosed in patent CN102531821, adopt the ZSM-5 catalyzer of load 2.2 ~ 6.0 % by weight La and 1.0 ~ 2.8 % by weight P, fixed-bed reactor or fluidized-bed reactor can be adopted.Temperature of reaction is 550 ~ 670 DEG C, air speed 1.0 ~ 5 (Grams Per Hour)/gram catalyzer.The triolefin yield of the method is higher, but BTX yield is low, only has 5 ~ 17 % by weight.
Patent CN102372537 and CN102190546 discloses the method for preparing propylene by methanol transformation and aromatic hydrocarbons.These two patents develop on the basis of preparing propylene by methanol transformation technology, and propylene is the product of argument, and aromatics yield is lower.
All there is technical process complexity in the patented technology of above-mentioned Methanol aromatic hydrocarbons, the problem that ethene, propene yield are low.In addition, for steam cracking process, ethene, propylene are main purpose products, and yield is higher than 40 % by weight, and aromatic hydrocarbons belongs to by product, and yield is 10 ~ 16 % by weight, lower, and product structure is difficult to adjust flexibly according to the market requirement.For this reason, propose technical scheme to the property of the present invention is directed to, solve the problems referred to above.
Summary of the invention
One of technical problem to be solved by this invention is that prior art Raw is single, and aromatics yield is low, and product structure can not, according to the problem of the flexible modulation of the market requirement, provide a kind of polymorphic type the material coupled system transforming ethene processed, propylene and aromatic hydrocarbons.This system has the advantage that aromatics yield is high, can adjust the product mix flexibly according to the market requirement.
Two of technical problem to be solved by this invention is to provide a kind of method corresponding with one of technical solution problem.
For one of solving the problem, the technical solution used in the present invention is as follows: the material coupled conversion of a kind of polymorphic type ethene processed, the system of propylene and aromatic hydrocarbons, comprise aromatization reactor 1, quench tower 2, knockout tower 3, steam cracking unit 4, the product that aromatization reactor 1 generates enters quench tower 2 and knockout tower 3 successively, the gaseous product that knockout tower 3 obtains enters the separation system of steam cracking unit 4 through compressor 5, the part ethane 20 that the separation system of knockout tower 3 and steam cracking unit 4 obtains, propane 21, C4 raffinate 27, C5 and C6 non-aromatic 11 returns aromatization reactor 1 as recycle stock.
In technique scheme, aromatization reactor 1, for methyl alcohol and/or dme and recycle stock being converted into, to comprise ethene, propylene and aromatic hydrocarbons be main product; Quench tower 2, the product that cooling aromatization reactor 1 generates; Knockout tower 3, is separated into the pyrolysis gasoline that quench tower 2 product out and steam cracking unit 4 obtain that water, hydrocarbon gas, C5 and C6 are non-aromatic, BTX aromatics; Steam cracking unit 4, by hydrocarbon raw material cracking, is separated into hydrogen, ethene, ethane, propylene, propane, divinyl, C4 raffinate, pyrolysis gasoline.
In technique scheme, methyl alcohol and/or dme and recycle stock are converted into the product comprising ethene, propylene and aromatic hydrocarbons at aromatization reactor 1; The product that aromatization reactor 1 generates cools in quench tower 2; The pyrolysis gasoline that quench tower 2 product out and steam cracking unit 4 obtain is separated in knockout tower 3 that water, hydrocarbon gas, C5 and C6 are non-aromatic, BTX aromatics; Hydrocarbon raw material in the cracking of steam cracking unit, and is separated into hydrogen, methane, ethene, ethane, propylene, propane, divinyl, C4 raffinate, pyrolysis gasoline.
For solve the problem two, the technical solution used in the present invention is as follows: a kind of polymorphic type is material coupled transforms the method for ethene processed, propylene and aromatic hydrocarbons, and adopt above-mentioned system, described method comprises following step:
A) methyl alcohol and/or dme and recycle stock are in aromatization reactor 1 and aromatized catalyst contact reacts, generate based on the product of ethene, propylene and aromatic hydrocarbons;
B) product that aromatization reactor 1 obtains enters quench tower 2 and cools;
C) knockout tower 3 is entered together with the pyrolysis gasoline 29 obtained through the cooled product of quench tower 2 and steam cracking unit 4, tower top isolates hydrocarbon gas, C5 and C6 non-aromatic 10 is isolated in the middle part of tower, isolate product at the bottom of tower and enter water-and-oil separator 6, be separated into BTX aromatics 8 and water 9, BTX aromatics 8 is as output of products system;
D) hydrocarbon gas is after compressor 5 pressurizes, and enters the separation system of steam cracking unit 4;
E) steam cracking unit 4 by hydrocarbon raw material cracking, be separated into hydrogen 13, methane 14, ethene 15, ethane 18, propylene 16, propane 19, divinyl 17, C4 raffinate 26, pyrolysis gasoline 29, wherein hydrogen 13, methane 14, ethene 15, propylene 16, divinyl 17 are as output of products system;
F) the part C5 that obtains of part ethane 20, propane 21, C4 raffinate 27 and knockout tower 3 and C6 non-aromatic 11 returns aromatization reactor 1 as recycle stock, part ethane 22, propane 23 return steam cracking unit 4 as recycle stock, remain ethane 24 or whole ethane 18, remain propane 25 or whole propane 19, residue C4 raffinate 28 or whole C4 raffinate 26, remain C5 and C6 non-aromatic 12 or whole C5 and C6 non-aromatic 10 as output of products system;
G) pyrolysis gasoline 29 that steam cracking unit 4 obtains enters knockout tower 3.
In technique scheme, aromatization reactor 1 adopts the circulating fluid bed reactor of fixed-bed reactor, moving-burden bed reactor, fluidized-bed reactor or band revivifier, the circulating fluid bed reactor of preferred fluidized-bed reactor or band revivifier.
In technique scheme, the active ingredient of aromatized catalyst is the composite molecular screen of ZSM-5, ZSM-23, ZSM-11, β, Y or formation each other; Carrier is kaolin, aluminum oxide, silicon-dioxide; The mass ratio of active ingredient and carrier is (10 ~ 50): (50 ~ 90).
In technique scheme, aromatized catalyst load has one or more elements or its oxide compound in Zn, Ag, P, Ga, Cu, Mn, Mg, and with the weight percent meter of catalyzer, its content is 0.01 ~ 15 % by weight.
In technique scheme, the active ingredient of aromatized catalyst is selected from ZSM-5 molecular sieve, with the weight percent meter of catalyzer, and the Zn element of load 0.01 ~ 5wt% or its oxide compound, the P element of 0.1 ~ 8wt% or its oxide compound on catalyzer.
In technique scheme, the temperature of reaction of aromatization reactor 1 is 400 ~ 550 DEG C, and in gauge pressure reaction pressure for 0 ~ 0.5MPa, weight space velocity is 0.1 ~ 15 h
-1, preferable reaction temperature is 440 ~ 500 DEG C, and in gauge pressure reaction pressure for 0.1 ~ 0.4MPa, weight space velocity is 0.1 ~ 10 h
-1.
In technique scheme, the hydrocarbon raw material of steam cracking unit can be ethane, propane, butane, pentane, petroleum naphtha, diesel oil, secondary processing oil, preferred ethane, propane, butane, pentane, petroleum naphtha.
In technique scheme, the separation system of steam cracking unit can be order separation process, predepropanization process and front-end deethanization flow process.
In technique scheme, the feed weight ratio of steam cracking unit and aromatization reactor is (10 ~ 90) ﹕ (90 ~ 10), can according to the market demand of ethene, propylene, aromatic hydrocarbons, the product structure of adjustment System is carried out by the material rate of steam regulation cracking technology and aromatization reactor, realize maximum ethene and propylene, maximum aromatic hydrocarbons, ethene, propylene and aromatic hydrocarbons coproduction three kinds of operator schemes.
Order separation process technical scheme provided by the invention: methyl alcohol and/or dme and recycle stock in aromatization reactor 1 and aromatized catalyst contact reacts, generate based on the product of ethene, propylene and aromatic hydrocarbons; The product that aromatization reactor 1 obtains enters quench tower 2 and cools; Knockout tower 3 is entered together with the pyrolysis gasoline 18 that the cooled product of quench tower 2 and steam cracking unit 4 obtain, tower top isolates hydrocarbon gas, C5 and C6 non-aromatic 10 is isolated in the middle part of tower, isolate product at the bottom of tower and enter water-and-oil separator 6, be separated into BTX aromatics 8 and water 9, BTX aromatics 8 is as output of products system; Part C5 and C6 non-aromatic 11 returns aromatization reactor 1, and residue C5 and C6 non-aromatic 12 or all C5 and C6 non-aromatic 10 are as output of products system; Hydrocarbon gas is after compressor 5 pressurizes, and enter the demethanizing tower 30 in steam cracking unit 4, demethanizing tower 30 tower top isolates hydrogen 13, methane 14, and bottom product enters deethanizing column 31; The C2 product introduction ethylene rectification tower 32 of deethanizing column 31 tower top, the carbon number at the bottom of tower enters depropanizing tower 33 higher than the hydrocarbon of more than 2; Ethylene rectification tower 32 tower top isolates ethene 15, isolates ethane 18 at the bottom of tower; The isolated C3 of depropanizing tower 33 tower top enters propylene rectification tower 34, and isolated carbon number at the bottom of tower enters debutanizing tower 35 higher than the hydrocarbon of 3; Debutanizing tower 35 tower top isolates hybrid C 4, isolates pyrolysis gasoline at the bottom of tower; Hybrid C 4 extracts after divinyl 17 through butadiene extraction unit 36 and obtains C4 raffinate 26; Propylene rectification tower 34 tower top isolates propylene 16, isolates propane 19 at the bottom of tower; Wherein hydrogen 13, methane 14, ethene 15, propylene 16, divinyl 17 are as output of products system; The part C5 that part ethane 20, propane 21, C4 raffinate 27 and knockout tower 3 obtain and C6 non-aromatic 11 returns aromatization reactor 1 as recycle stock, part ethane 22, propane 23 return steam cracking unit 4 as recycle stock, remain ethane 24 or whole ethane 18, remain propane 25 or whole propane 19, residue C4 raffinate 28 or whole C4 raffinate 26, remain C5 and C6 non-aromatic 12 or whole C5 and C6 non-aromatic 10 as output of products system.
Front-end deethanization flow technologies scheme provided by the invention: methyl alcohol and/or dme and recycle stock in aromatization reactor 1 and aromatized catalyst contact reacts, generate based on the product of ethene, propylene and aromatic hydrocarbons; The product that aromatization reactor 1 obtains enters quench tower 2 and cools; Knockout tower 3 is entered together with the pyrolysis gasoline 29 that the cooled product of quench tower 2 and steam cracking unit 4 obtain, tower top isolates hydrocarbon gas, C5 and C6 non-aromatic 10 is isolated in the middle part of tower, isolate product at the bottom of tower and enter water-and-oil separator 6, be separated into BTX aromatics 8 and water 9, BTX aromatics 8 is as output of products system; Part C5 and C6 non-aromatic 11 returns aromatization reactor 1, and residue C5 and C6 non-aromatic 12 or all C5 and C6 non-aromatic 10 are as output of products system; Hydrocarbon gas, after compressor 5 pressurizes, enters the deethanizing column 31 in steam cracking unit 4; The product introduction demethanizing tower 30 of deethanizing column 35 tower top, bottom product enters depropanizing tower 33; Demethanizing tower 30 tower top isolates hydrogen 13, methane 14, and bottom product enters ethylene rectification tower 32; Ethylene rectification tower 32 tower top isolates ethene 15, isolates ethane 18 at the bottom of tower; The isolated C3 of depropanizing tower 33 tower top enters propylene rectification tower 34, and isolated carbon number at the bottom of tower enters debutanizing tower 35 higher than the hydrocarbon of 3; Debutanizing tower 35 tower top isolates hybrid C 4, isolates pyrolysis gasoline at the bottom of tower; Hybrid C 4 extracts after divinyl 17 through butadiene extraction unit 36 and obtains C4 raffinate 26; Propylene rectification tower 34 tower top isolates propylene 16, isolates propane 19 at the bottom of tower; Wherein hydrogen 13, methane 14, ethene 15, propylene 16, divinyl 17 are as output of products system; The part C5 that part ethane 20, propane 21, C4 raffinate 27 and knockout tower 3 obtain and C6 non-aromatic (11) returns aromatization reactor 1 as recycle stock, part ethane 22, propane 23 return steam cracking unit 4 as recycle stock, remain ethane 24 or whole ethane 18, remain propane 25 or whole propane 19, residue C4 raffinate 28 or whole C4 raffinate 26, remain C5 and C6 non-aromatic 12 or whole C5 and C6 non-aromatic 10 as output of products system.
Predepropanization process technical scheme provided by the invention: methyl alcohol and/or dme and recycle stock in aromatization reactor 1 and aromatized catalyst contact reacts, generate based on the product of ethene, propylene and aromatic hydrocarbons; The product that aromatization reactor 1 obtains enters quench tower 2 and cools; Knockout tower 3 is entered together with the pyrolysis gasoline 29 that the cooled product of quench tower 2 and steam cracking unit 4 obtain, tower top isolates hydrocarbon gas, C5 and C6 non-aromatic 10 is isolated in the middle part of tower, isolate product at the bottom of tower and enter water-and-oil separator 6, be separated into BTX aromatics 8 and water 9, BTX aromatics 8 is as output of products system; Part C5 and C6 non-aromatic 11 returns aromatization reactor 1, and residue C5 and C6 non-aromatic 12 or all C5 and C6 non-aromatic 10 are as output of products system; Hydrocarbon gas, after compressor 5 pressurizes, enters the depropanizing tower 33 in steam cracking unit 4; The product introduction demethanizing tower 30 of depropanizing tower 33 tower top, isolated carbon number at the bottom of tower enters debutanizing tower 35 higher than the hydrocarbon of 3; Debutanizing tower 35 tower top isolates hybrid C 4, isolates pyrolysis gasoline at the bottom of tower; Hybrid C 4 extracts after divinyl 17 through butadiene extraction unit 36 and obtains C4 raffinate 26; Demethanizing tower 30 tower top isolates hydrogen 13, methane 14, and bottom product enters deethanizing column 31; The C2 product introduction ethylene rectification tower 32 of deethanizing column 31 tower top, the carbon number at the bottom of tower enters propylene rectification tower 34 higher than the hydrocarbon of 2; Ethylene rectification tower 32 tower top isolates ethene 15, isolates ethane 18 at the bottom of tower; Propylene rectification tower 34 tower top isolates propylene 16, isolates propane 19 at the bottom of tower; Wherein hydrogen 13, methane 14, ethene 15, propylene 16, divinyl 17 are as output of products system; The part C5 that part ethane 20, propane 21, C4 raffinate 27 and knockout tower 3 obtain and C6 non-aromatic 11 returns aromatization reactor 1 as recycle stock, part ethane 22, propane 23 return steam cracking unit 4 as recycle stock, remain ethane 24 or whole ethane 18, remain propane 25 or whole propane 19, residue C4 raffinate 28 or whole C4 raffinate 26, remain C5 and C6 non-aromatic 12 or whole C5 and C6 non-aromatic 10 as output of products system.
The present invention is by being organically coupled preparing ethylene by steam cracking, propylene process and methyl alcohol and/or dimethyl ether conversion aromatic hydrocarbons process, give full play to the advantage of two processes respectively in ethene, production of propylene and aromatics production, realize the object that ethene, propylene and aromatics yield are high.Meanwhile, can also according to the market requirement of ethene, propylene, aromatic hydrocarbons, the production load of adjustment two processes, realizes maximization of economic benefit.Because two process products composition has certain general character, two reaction process common sparing separation systems in the present invention, can effective investment reduction, realize energy-saving and emission-reduction.
Adopt order separation process technical scheme of the present invention, described aromatization reactor adopts the circulating fluid bed reactor of band revivifier; The temperature of reaction of described aromatization reactor is 480 DEG C, and in gauge pressure reaction pressure for 0.13MPa, weight space velocity is 1 h
-1; The active ingredient of described aromatized catalyst is ZSM-5 molecular sieve, and content is on a catalyst 35 % by weight, catalyst cupport Zn, P, and content is on a catalyst respectively 5% weight and 3 % by weight; Described steam cracking unit adopts naphtha feed, and aromatization reactor adopts methanol feeding, and feed weight is than being 50:50; The cracking temperature of described steam cracking unit is 950 DEG C.Ethene+propylene total recovery can reach 53% weight, and aromatics yield is 35 % by weight, BTX yields is 25 % by weight, achieves good technique effect.
Accompanying drawing explanation
Fig. 1 is the schematic flow sheet of technical scheme of the present invention.
Fig. 2 is the separation system schematic flow sheet of steam cracking unit 4 in order separation process technical scheme of the present invention;
Fig. 3 is the separation system schematic flow sheet of steam cracking unit 4 in front-end deethanization flow technologies scheme of the present invention;
Fig. 4 is the separation system schematic flow sheet of steam cracking unit 4 in predepropanization process technical scheme of the present invention.
In Fig. 1 ~ 4,1 is aromatization reactor; 2 is quench tower; 3 is knockout tower; 4 is steam cracking unit; 5 is compressor; 6 is water-and-oil separator; 7 is methyl alcohol and/or dme; 8 is BTX aromatics; 9 is water; 10 is that C5 and C6 is non-aromatic; 11 for C5 and C6 returning aromatization reactor non-aromatic; 12 is that C5 and C6 of output system is non-aromatic; 13 is hydrogen; 14 is methane; 15 is ethene; 16 is propylene; 17 is divinyl; 18 is ethane; 19 is propane; 20 for returning the ethane of aromatization reactor; 21 for returning the propane of aromatization reactor; 22 for returning the ethane of steam cracking unit; 23 for returning the propane of steam cracking unit; 24 is the ethane of output system; 25 is the propane of output system; 26 is C4 raffinate; 27 for returning the C4 raffinate of aromatization reactor; 28 is the C4 raffinate of output system; 29 is pyrolysis gasoline; 30 is demethanizing tower; 31 is deethanizing column; 32 is ethylene rectification tower; 33 is depropanizing tower; 34 is propylene rectification tower; 35 is debutanizing tower; 36 butadiene extraction unit.
In Fig. 1, methyl alcohol and/or dme and recycle stock are in aromatization reactor 1 and aromatized catalyst contact reacts, generate based on the product of ethene, propylene and aromatic hydrocarbons; The product that aromatization reactor 1 obtains enters quench tower 2 and cools; Knockout tower 3 is entered together with the pyrolysis gasoline 29 that the cooled product of quench tower 2 and steam cracking unit 4 obtain, tower top isolates hydrocarbon gas, C5 and C6 non-aromatic 10 is isolated in the middle part of tower, isolate product at the bottom of tower and enter water-and-oil separator 6, be separated into BTX aromatics 8 and water 9, BTX aromatics 8 is as output of products system; Hydrocarbon gas, after compressor 5 pressurizes, enters the separation system of steam cracking unit 4; Steam cracking unit 4 by hydrocarbon raw material cracking, be separated into hydrogen 13, methane 14, ethene 15, ethane 18, propylene 16, propane 19, divinyl 17, C4 raffinate 26, pyrolysis gasoline 29, wherein hydrogen 13, methane 14, ethene 15, propylene 16, divinyl 17 are as output of products system; The part C5 that part ethane 20, propane 21, C4 raffinate 27 and knockout tower 3 obtain and C6 non-aromatic 11 returns aromatization reactor 1 as recycle stock, part ethane 22, propane 23 return steam cracking unit 4 as recycle stock, remain ethane 24 or whole ethane 18, remain propane 25 or whole propane 19, residue C4 raffinate 28 or whole C4 raffinate 26, remain C5 and C6 non-aromatic 12 or whole C5 and C6 non-aromatic 10 as output of products system; The pyrolysis gasoline 29 that steam cracking unit 4 obtains enters knockout tower 3.
The product compressed through compressor 5 in Fig. 2 enters the demethanizing tower 30 in steam cracking unit 4, and demethanizing tower 30 tower top isolates hydrogen 13, methane 14, and bottom product enters deethanizing column 31; The C2 product introduction ethylene rectification tower 32 of deethanizing column 31 tower top, the carbon number at the bottom of tower enters depropanizing tower 33 higher than the hydrocarbon of more than 2; Ethylene rectification tower 32 tower top isolates ethene 15, isolates ethane 18 at the bottom of tower; The isolated C3 of depropanizing tower 33 tower top enters propylene rectification tower 34, and isolated carbon number at the bottom of tower enters debutanizing tower 35 higher than the hydrocarbon of 3; Debutanizing tower 35 tower top isolates hybrid C 4, isolates pyrolysis gasoline at the bottom of tower; Hybrid C 4 extracts after divinyl 17 through butadiene extraction unit 36 and obtains C4 raffinate 26; Propylene rectification tower 34 tower top isolates propylene 16, isolates propane 19 at the bottom of tower.
The product compressed through compressor 5 in Fig. 3 enters the deethanizing column 31 in steam cracking unit 4; The product introduction demethanizing tower 30 of deethanizing column 35 tower top, bottom product enters depropanizing tower 33; Demethanizing tower 30 tower top isolates hydrogen 13, methane 14, and bottom product enters ethylene rectification tower 32; Ethylene rectification tower 32 tower top isolates ethene 15, isolates ethane 18 at the bottom of tower; The isolated C3 of depropanizing tower 33 tower top enters propylene rectification tower 34, and isolated carbon number at the bottom of tower enters debutanizing tower 35 higher than the hydrocarbon of 3; Debutanizing tower 35 tower top isolates hybrid C 4, isolates pyrolysis gasoline at the bottom of tower; Hybrid C 4 extracts after divinyl 17 through butadiene extraction unit 36 and obtains C4 raffinate 26; Propylene rectification tower 34 tower top isolates propylene 16, isolates propane 19 at the bottom of tower.
The product compressed through compressor 5 in Fig. 4 enters the depropanizing tower 33 in steam cracking unit 4; The product introduction demethanizing tower 30 of depropanizing tower 33 tower top, isolated carbon number at the bottom of tower enters debutanizing tower 35 higher than the hydrocarbon of 3; Debutanizing tower 35 tower top isolates hybrid C 4, isolates pyrolysis gasoline at the bottom of tower; Hybrid C 4 extracts after divinyl 17 through butadiene extraction unit 36 and obtains C4 raffinate 26; Demethanizing tower 30 tower top isolates hydrogen 13, methane 14, and bottom product enters deethanizing column 31; The C2 product introduction ethylene rectification tower 32 of deethanizing column 31 tower top, the carbon number at the bottom of tower enters propylene rectification tower 34 higher than the hydrocarbon of 2; Ethylene rectification tower 32 tower top isolates ethene 15, isolates ethane 18 at the bottom of tower; Propylene rectification tower 34 tower top isolates propylene 16, isolates propane 19 at the bottom of tower.
Below by embodiment, the invention will be further elaborated.
Embodiment
[embodiment 1]
The technical scheme of employing order separation process.
Aromatization reactor adopts circulating fluid bed reactor.The operation steps of this device comprises: (1) raw material enters in reactor, with regenerated catalyst contact reacts, generates the product containing low-carbon alkene, carries reclaimable catalyst and enter settling vessel through gas-solid quick disconnector; (2) most of catalyzer that cyclonic separator is separated enters settling vessel, and gaseous products and part are not entered next stage cyclonic separator by the catalyzer that cyclonic separator is separated and be again separated; (3) gaseous products enters follow-up separate part through outlet line; (4) in settling vessel, reclaimable catalyst is through inclined tube to be generated and guiding valve to be generated after stripping stage stripping, and enter coke-burning regeneration in revivifier, the flue gas that coke burning generates discharges system through revivifier internal cyclone separators; (5) catalyzer regenerated enters in reactor and participates in reaction.
The reaction conditions of aromatization reactor is: temperature 480 DEG C, in gauge pressure reaction pressure 0.3 MPa, and weight space velocity 0.5 (Grams Per Hour)/gram catalyzer.Take methyl alcohol as raw material, adopt Cu-ZSM-5 catalyzer.
The preparation process of Cu-ZSM-5 catalyzer: by ZSM-5 molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, HCl, controls pH value and is not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object ZSM-5 catalyst intermediate.The mass ratio of ZSM-5 molecular sieve and matrix is 4:6; The silicoaluminophosphate molecular ratio of ZSM-5 molecular sieve is 25; Matrix is the mixture of kaolin and aluminium sesquioxide, and both mass ratioes are 7:3.Be the solution of 5% by Cu mass of ion percentage composition, with the weight ratio of solution and catalyzer for 1.74:1 floods, at 120 DEG C dry 5 hours, then put into retort furnace roasting at 550 DEG C and within 6 hours, be prepared into the Cu-ZSM-5 catalyzer that Cu constituent content is 8 % by weight.
Steam cracking unit take petroleum naphtha as raw material, and cracking temperature is 900 DEG C, and steam and raw materials quality ratio are 0.4.
The feed weight of steam cracking unit and aromatization reactor is than being 90:10, and reaction result is listed in table 1.
[embodiment 2]
Adopt the aromatization reactor in front-end deethanization flow technologies scheme and embodiment 1.
The reaction conditions of aromatization reactor is: temperature 550 DEG C, in gauge pressure reaction pressure 0.5 MPa, and weight space velocity 15 (Grams Per Hour)/gram catalyzer.Take dme as raw material, adopt Ag-Y-ZSM-23 catalyzer.
The preparation process of Ag-Y-ZSM-23 catalyzer: by Y molecular sieve, ZSM-23 molecular screen, carrier and binding agent mechanically mixing, add suitable quantity of water, HCl, control pH value and be not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object Y-ZSM-23 catalyst intermediate.The mass ratio of molecular sieve and matrix is 1:9; Y molecular sieve and ZSM-23 molecular screen mass ratio are 3:7; The silicoaluminophosphate molecular ratio of Y molecular sieve is 10; The silicoaluminophosphate molecular ratio of ZSM-23 molecular screen is 60; Matrix is the mixture of kaolin and aluminium sesquioxide, and both mass ratioes are 8:2.Be the solution of 1% by Ag mass of ion percentage composition, flood than for 0.1:1 with solution and catalyst weight, at 120 DEG C dry 5 hours, then put into retort furnace roasting at 550 DEG C and within 6 hours, be prepared into the Ag-Y-ZSM-23 catalyzer that Ag constituent content is 0.1 % by weight.
Steam cracking unit take butane as raw material, and cracking temperature is 970 DEG C, and steam and raw materials quality ratio are 0.1.
The feed weight of steam cracking unit and aromatization reactor is than being 60:40, and reaction result is listed in table 1.
[embodiment 3]
Adopt the aromatization reactor in predepropanization technical scheme and embodiment 1.
The reaction conditions of aromatization reactor is: temperature 400 DEG C, in gauge pressure reaction pressure 0 MPa, and weight space velocity 0.1 (Grams Per Hour)/gram catalyzer.Take dme as raw material, adopt Ga-beta catalyst.
The preparation process of Ga-beta catalyst: by beta-molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, HCl, controls pH value and is not less than 4, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object beta catalyst intermediates.The mass ratio of beta-molecular sieve and matrix is 5:5; The silicoaluminophosphate molecular ratio of beta-molecular sieve is 20; Matrix is the mixture of kaolin, silicon-dioxide and aluminium sesquioxide, and the mass ratio of three is 7:1:2.Be the solution of 2% by Ga mass of ion percentage composition, flood than for 0.4:1 with solution and catalyst weight, at 120 DEG C dry 5 hours, then put into retort furnace roasting at 550 DEG C and within 6 hours, be prepared into the Ga-beta catalyst that Ga constituent content is 0.8 % by weight.
Steam cracking unit take propane as raw material, and cracking temperature is 1000 DEG C, and steam and raw materials quality ratio are 0.08.
The feed weight of steam cracking unit and aromatization reactor is than being 80:20, and reaction result is listed in table 1.
[embodiment 4]
Employing order separation process technical scheme.
Aromatization reactor is fixed-bed reactor.Beds is positioned in the middle part of reactor, and reaction raw materials enters in reactor from top to bottom and reacts.
The reaction conditions of aromatization reactor is: temperature 500 DEG C, in gauge pressure reaction pressure 0.25 MPa, and weight space velocity 1 (Grams Per Hour)/gram catalyzer.Take methyl alcohol as raw material, adopt Mn-ZSM-11 catalyzer.
The preparation process of Mn-ZSM-11 catalyzer: by ZSM-11 molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, HCl, control pH value and be not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object ZSM-11 catalyst intermediate.The mass ratio of ZSM-11 molecular sieve and matrix is 3:7; The silicoaluminophosphate molecular ratio of ZSM-11 molecular sieve is 50; Matrix is the mixture of kaolin and aluminium sesquioxide, and both mass ratioes are 7:3.Be the solution of 10% by Mn mass of ion percentage composition, with the weight ratio of solution and catalyzer for 1:1 floods, at 120 DEG C dry 5 hours, then put into retort furnace roasting at 550 DEG C and within 6 hours, be prepared into the Mn-ZSM-11 catalyzer that Mn constituent content is 9.09 % by weight.
Steam cracking unit take ethane as raw material, and cracking temperature is 1200 DEG C, and steam and raw materials quality ratio are 0.08.
The feed weight of steam cracking unit and aromatization reactor is than being 70:30, and reaction result is listed in table 1.
[embodiment 5]
Adopt the aromatization reactor in front-end deethanization flow technologies scheme and embodiment 1.
The reaction conditions of aromatization reactor is: temperature 480 DEG C, in gauge pressure reaction pressure 0.3 MPa, and weight space velocity 2 (Grams Per Hour)/gram catalyzer.Take methyl alcohol as raw material, adopt Zn-P-ZSM-5 catalyzer.
The preparation process of Zn-P-ZSM-5 catalyzer: by ZSM-5 molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, H
3pO
4, control pH value and be not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object P-ZSM-5 catalyst intermediate.H
3pO
4the concentration of solution is 1 % by weight, and the weight ratio of solution and molecular sieve is 1.53:1.The mass ratio of ZSM-5 molecular sieve and matrix is 3.5:6.5; The silicoaluminophosphate molecular ratio of ZSM-5 molecular sieve is 25; Matrix is the mixture of kaolin and aluminium sesquioxide, and both mass ratioes are 7:3.Be the solution of 5% by Zn mass of ion percentage composition, flood than for 0.6:1 with solution and P-ZSM-5 catalyst weight, drying 5 hours at 120 DEG C, put into retort furnace roasting 6 hours at 550 DEG C again, being prepared into Zn constituent content is 2.87 % by weight, and P element content is the Zn-P-ZSM-5 catalyzer of 1.48 % by weight.
Steam cracking unit take diesel oil as raw material, and cracking temperature is 1100 DEG C, and steam and raw materials quality ratio are 0.1.
The feed weight of anti-steam cracking unit and aromatization reactor, should the results are shown in Table 1 than being 10:90.
[embodiment 6]
Adopt the aromatization reactor in predepropanization technical scheme and embodiment 4.
The reaction conditions of aromatization reactor is: temperature 470 DEG C, in gauge pressure reaction pressure 0.4 MPa, and weight space velocity 5 (Grams Per Hour)/gram catalyzer.Take methyl alcohol as raw material, adopt ZSM-5-beta catalyst.
The preparation process of ZSM-5-beta catalyst: by ZSM-5 molecular sieve, beta-molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, HCl, control pH value and be not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object ZSM-5-beta catalysts.The mass ratio of ZSM-5 and beta-molecular sieve and matrix is 3.5: 6.5.The silicoaluminophosphate molecular ratio of ZSM-5 molecular sieve is 38; The silicoaluminophosphate molecular ratio of beta-molecular sieve is 20; The mass ratio of ZSM-5 and beta-molecular sieve is 9:1.Matrix is the mixture of kaolin, silicon-dioxide and aluminium sesquioxide, and the mass ratio of three is 5:2:3.
Steam cracking unit take pentane as raw material, and cracking temperature is 1000 DEG C, and steam and raw materials quality ratio are 0.12.
The feed weight of steam cracking unit and aromatization reactor is than being 40:60, and reaction result is listed in table 1.
[embodiment 7]
Employing order separation process technical scheme and embodiment 1 in aromatization reactor.
The reaction conditions of aromatization reactor is: temperature 500 DEG C, in gauge pressure reaction pressure 0.3 MPa, and weight space velocity 3 (Grams Per Hour)/gram catalyzer.Take methyl alcohol as raw material, adopt Zn-Ag-P-ZSM-5 catalyzer.
The preparation process of Zn-Ag-P-ZSM-5 catalyzer: by ZSM-5 molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, H
3pO
4, control pH value and be not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object P-ZSM-5 catalyst intermediate.H
3pO
4the concentration of solution is 2.5 % by weight, and the weight ratio of solution and molecular sieve is 2:1.The mass ratio of ZSM-5 molecular sieve and matrix is 3.5:6.5; The silicoaluminophosphate molecular ratio of ZSM-5 molecular sieve is 28; Matrix is the mixture of kaolin and aluminium sesquioxide, and both mass ratioes are 8:2.Be 1% by Ag mass of ion percentage composition, Zn mass of ion percentage composition is the solution of 3%, flood than for 0.8:1 with solution and P-ZSM-5 catalyst weight, drying 5 hours at 120 DEG C, put into retort furnace roasting 6 hours at 550 DEG C again, being prepared into Zn constituent content is 2.32 % by weight, Ag constituent content is 0.78 % by weight, and P element content is the Zn-Ag-P-ZSM-5 catalyzer of 1.51 % by weight.
Steam cracking unit take petroleum naphtha as raw material, and cracking temperature is 920 DEG C, and steam and raw materials quality ratio are 0.35.
The feed weight of steam cracking unit and aromatization reactor is than being 50:50, and reaction result is listed in table 1.
[embodiment 8]
Adopt the aromatization reactor in front-end deethanization flow technologies scheme and embodiment 1.
The reaction conditions of aromatization reactor is: temperature 470 DEG C, in gauge pressure reaction pressure 0.25 MPa, and weight space velocity 0.5 (Grams Per Hour)/gram catalyzer.Take methyl alcohol as raw material, adopt Zn-Mg-P-ZSM-5 catalyzer.
The preparation process of Zn-Mg-P-ZSM-5 catalyzer: by ZSM-5 molecular sieve, carrier and binding agent mechanically mixing, add suitable quantity of water, H
3pO
4, control pH value and be not less than 3, slurry agitation evenly after at 500 DEG C spray shaping, make 60 ~ 300 object P-ZSM-5 catalyst intermediate.H
3pO
4the concentration of solution is 4 % by weight, and the weight ratio of solution and molecular sieve is 2:1.The mass ratio of ZSM-5 molecular sieve and matrix is 3:7; The silicoaluminophosphate molecular ratio of ZSM-5 molecular sieve is 32; Matrix is the mixture of kaolin and aluminium sesquioxide, and both mass ratioes are 7:3.Be 2% by Mg mass of ion percentage composition, Zn mass of ion percentage composition is the solution of 3%, flood than for 1:1 with solution and P-ZSM-5 catalyst weight, drying 5 hours at 120 DEG C, put into retort furnace roasting 6 hours at 550 DEG C again, being prepared into Zn constituent content is 2.86 % by weight, Mg constituent content is 1.9 % by weight, and P element content is the Zn-Mg-P-ZSM-5 catalyzer of 2.35 % by weight.
Steam cracking unit is with secondary processing oil for raw material, and cracking temperature is 850 DEG C, and steam and raw materials quality ratio are 0.5.
The feed weight of steam cracking unit and aromatization reactor is than being 30:70, and reaction result is listed in table 1.
Table 1
| Yield of ethene, % by weight | Propene yield, % by weight | Aromatics yield, % by weight | |
| Embodiment 1 | 31.6 | 10.8 | 14.1 |
| Embodiment 2 | 20.3 | 10.0 | 12.7 |
| Embodiment 3 | 8.09 | 24 | 6.9 |
| Embodiment 4 | 35.3 | 1.53 | 9.45 |
| Embodiment 5 | 3.59 | 1.79 | 30.94 |
| Embodiment 6 | 14.26 | 6 | 22.49 |
| Embodiment 7 | 15.22 | 7.72 | 23.63 |
| Embodiment 8 | 8.41 | 4.51 | 28.06 |
Claims (10)
1. the material coupled conversion of a polymorphic type ethene processed, the system of propylene and aromatic hydrocarbons, comprise aromatization reactor (1), quench tower (2), knockout tower (3), steam cracking unit (4), the product that aromatization reactor (1) generates enters quench tower (2) and knockout tower (3) successively, the gaseous product that knockout tower (3) obtains enters the separation system of steam cracking unit (4) through compressor (5), the part ethane (20) that the separation system of knockout tower (3) and steam cracking unit (4) obtains, propane (21), C4 raffinate (27), C5 and C6 non-aromatic (11) returns aromatization reactor (1) as recycle stock.
2. polymorphic type according to claim 1 is material coupled transforms the system of ethene processed, propylene and aromatic hydrocarbons, it is characterized in that: methyl alcohol and/or dme and recycle stock are converted at aromatization reactor (1) product comprising ethene, propylene and aromatic hydrocarbons; The product that aromatization reactor (1) generates is cooling in quench tower (2); The pyrolysis gasoline that quench tower (2) product out and steam cracking unit (4) obtain is separated in knockout tower (3) that water, hydrocarbon gas, C5 and C6 are non-aromatic, BTX aromatics; Hydrocarbon raw material in the cracking of steam cracking unit, and is separated into hydrogen, methane, ethene, ethane, propylene, propane, divinyl, C4 raffinate, pyrolysis gasoline.
3. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type, adopt the system described in claim 1 or 2, described method comprises following step:
A) methyl alcohol and/or dme and recycle stock are in aromatization reactor (1) and aromatized catalyst contact reacts, generate based on the product of ethene, propylene and aromatic hydrocarbons;
B) product that aromatization reactor (1) obtains enters quench tower (2) cooling;
C) knockout tower (3) is entered together with the pyrolysis gasoline (29) obtained through quench tower (2) cooled product and steam cracking unit (4), tower top isolates hydrocarbon gas, C5 and C6 non-aromatic (10) is isolated in the middle part of tower, isolate product at the bottom of tower and enter water-and-oil separator (6), be separated into BTX aromatics (8) and water (9), BTX aromatics (8) is as output of products system;
D) hydrocarbon gas is after compressor (5) pressurization, enters the separation system of steam cracking unit (4);
E) steam cracking unit (4) by hydrocarbon raw material cracking, be separated into hydrogen (13), methane (14), ethene (15), ethane (18), propylene (16), propane (19), divinyl (17), C4 raffinate (26), pyrolysis gasoline (29), wherein hydrogen (13), methane (14), ethene (15), propylene (16), divinyl (17) are as output of products system;
F) the part C5 that obtains of part ethane (20), propane (21), C4 raffinate (27) and knockout tower (3) and C6 non-aromatic (11) returns aromatization reactor (1) as recycle stock, part ethane (22), propane (23) return steam cracking unit (4) as recycle stock, remain ethane (24) or whole ethane (18), remain propane (25) or whole propane (19), residue C4 raffinate (28) or whole C4 raffinate (26), remain C5 and C6 non-aromatic (12) or whole C5 and C6 non-aromatic (10) as output of products system;
G) pyrolysis gasoline (29) that steam cracking unit (4) obtains enters knockout tower (3).
4. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 3, is characterized in that aromatization reactor (1) adopts the circulating fluid bed reactor of fixed-bed reactor, moving-burden bed reactor, fluidized-bed reactor or band revivifier.
5. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 3, is characterized in that the active ingredient of aromatized catalyst is ZSM-5, ZSM-23, ZSM-11, β zeolite, Y zeolite or the mutual composite molecular screen formed; Carrier is kaolin, aluminum oxide, silicon-dioxide; The mass ratio of active ingredient and carrier is (10 ~ 50): (50 ~ 90).
6. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 5, it is characterized in that aromatized catalyst load has one or more elements or its oxide compound in Zn, Ag, P, Ga, Cu, Mn, Mg, with the weight percent meter of catalyzer, its content is 0.01 ~ 15 % by weight.
7. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 5, it is characterized in that the active ingredient of aromatized catalyst is selected from ZSM-5 molecular sieve, with the weight percent meter of catalyzer, the Zn element of load 0.01 ~ 5 % by weight on catalyzer or its oxide compound, the P element of 0.1 ~ 8 % by weight or its oxide compound.
8. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 3, it is characterized in that the temperature of reaction of aromatization reactor (1) is 400 ~ 550 DEG C, in gauge pressure reaction pressure for 0 ~ 0.5MPa, weight space velocity is 0.1 ~ 15 h
-1.
9. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 3, is characterized in that the feed weight ratio of steam cracking unit (4) and aromatization reactor (1) is for (10 ~ 90): (90 ~ 10).
10. the material coupled method transforming ethene processed, propylene and aromatic hydrocarbons of polymorphic type according to claim 6, it is characterized in that the temperature of reaction of aromatization reactor (1) is 440 ~ 500 DEG C, be 0.1 ~ 0.4 MPa in gauge pressure reaction pressure, weight space velocity is 0.1 ~ 10 h
-1.
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